Water Concentration in Single‐Crystal (Al,Fe)‐Bearing
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RESEARCH LETTER Water Concentration in Single‐Crystal (Al,Fe)‐Bearing 10.1029/2019GL084630 Bridgmanite Grown From the Hydrous Melt: Implications Key Points: • High‐quality, inclusion‐free for Dehydration Melting at the Topmost Lower Mantle bridgmanite single crystals Suyu Fu1 , Jing Yang1,2 , Shun‐ichiro Karato3 , Alexander Vasiliev4,5,6, (Mg Fe3+ Fe2+ Al Si O ) 0.88 0.065 0.035 0.14 0.90 3 4 6,7,8 6,7 were synthesized and characterized Mikhail Yu. Presniakov , Alexander G. Gavrilliuk , Anna G. Ivanova , • The crystals contain ~1,020(±70) Erik H. Hauri9,10 , Takuo Okuchi11 , Narangoo Purevjav11 , and Jung‐Fu Lin1 ppm wt water using NanoSIMS and show pronounced OH‐stretching 1Department of Geological Sciences, Jackson School of Geosciences, The University of Texas at Austin, Austin, TX, USA, ‐1 bands at ~3230 and ~3460 cm in 2Geophysical Laboratory, Carnegie Institution of Washington, Washington, DC, USA, 3Department of Geology and FTIR spectra 4 • Dehydration melting at the topmost Geophysics, Yale University, New Haven, CT, USA, National Research Center, Kurchatov Institute, Moscow, Russia, 5 6 lower mantle can occur when water Moscow Institute of Physics and Technology, Moscow, Russia, Shubnikov Institute of Crystallography of Federal content exceeds ~0.1 wt% solubility Scientific Research Center Crystallography and Photonics, Russian Academy of Sciences, Moscow, Russia, 7Institute for limit Nuclear Research, Russian Academy of Science, Moscow, Russia, 8REC Functional Nanomaterials, Immanuel Kant Baltic Federal University, Kaliningrad, Russia, 9Department of Terrestrial Magnetism, Carnegie Institution of Washington, Supporting Information: Washington, DC, USA, 10Deceased, 11Institute for Planetary Materials, Okayama University, Misasa, Japan • Supporting Information S1 • Data Set S1 3+ 2+ Abstract High‐quality single‐crystals of (Al,Fe)‐bearing bridgmanite, Mg0.88 Fe 0.065Fe 0.035Al0.14Si0.90O3, of hundreds of micrometer size were synthesizedat24GPaand1800°CinaKawai‐type apparatus from the Correspondence to: J.‐F. Lin and S.‐i. Karato, starting hydrous melt containing ~6.7 wt% water. Analyses of synthesized bridgmanite using petrographic [email protected]; microscopy, scanning electron microscopy, and transmission electron microscopy show that the crystals are ‐ shun [email protected] chemically homogeneous and inclusion free in micrometer‐ to nanometer‐spatial resolutions. Nanosecondary ion mass spectrometry (NanoSIMS) analyses on selected platelets show ~1,020(±70) ppm wt water Citation: (hydrogen). The high water concentration in the structure of bridgmanite was further confirmed using ‐ Fu, S., Yang, J., Karato, S. i., Vasiliev, polarized and unpolarized Fourier‐transform infrared spectroscopy (FTIR) analyses with two pronounced A., Presniakov, M. Y., Gavrilliuk, A. G., ‐ −1 ‐ et al. (2019). Water concentration in OH stretching bands at ~3,230 and ~3,460 cm .Ourresultsindicatethatlowermantle bridgmanite can single‐crystal (Al,Fe)‐bearing accommodate relatively high amount of water. Therefore, dehydration melting at the topmost lower bridgmanite grown from the hydrous mantle by downward flow of transition zone materials would require water content exceeding melt: Implications for dehydration melting at the topmost lower mantle. ~0.1 wt%. Geophysical Research Letters, 46. https://doi.org/10.1029/2019GL084630 Plain Language Summary Water cycle between surface oceans and Earth's deep interior is a key to understanding the evolution and physical/chemical states of the planet. Early studies show that Received 19 JUL 2019 major transition zone minerals, wadsleyite, and ringwoodite, could accommodate abundant water (1–3 Accepted 12 AUG 2019 wt%), in the form of lattice‐bonded hydrogen atoms, in their crystal structures. However, water solubility in Accepted article online 16 AUG 2019 lower‐mantle bridgmanite, the most abundant mineral in the most volumetric layer of the planet, has remained poorly understood. The scientific challenge here was largely due to difficulties in making large‐ sized high‐quality single‐crystals of bridgmanite for reliable characterizations of its water concentration. Here we synthesized single‐crystal bridgmanite of a few hundred micrometers in diameter, which are examined to be inclusion and precipitate free and thus can be used for reliable water concentration measurements using NanoSIMS analyses. Unpolarized and polarized FTIR analyses are used to identify characteristic OH‐stretching bands. Our results show that (Al,Fe)‐bearing bridgmanite could contain as high as 1,020(±70) ppm wt water. This high water concentration in bridgmanite has implications for our understanding of how melting can occur deep in the mantle below the transition zone. 1. Introduction Water (hydrogen) can be dissolved into the structures of most mantle minerals including those that nominally do not have hydrogen in their chemical formulae such as olivine and its high‐pressure polymorphs, wadsleyite, and ringwoodite, (Mg,Fe)2SiO4, called as nominally anhydrous minerals (NAMs; e.g., Bolfan‐Casanova, 2005; Karato, 2015; Peslier et al., 2017). Water in NAMs can have significant effects ©2019. American Geophysical Union. on a variety of properties, including melting relationships (Inoue, 1994; Kawamoto, 2004), rheological All Rights Reserved. properties (Karato & Jung, 2003; Mei & Kohlstedt, 2000), and electrical conductivity (Karato & Wang, FU ET AL. 1 Geophysical Research Letters 10.1029/2019GL084630 2013). For instance, early studies indicate that partial or dehydration melting would occur when water‐rich materials in the transition zone such as wadsleyite or ringwoodite are transported to either upper or lower mantle regions where water solubility is low (e.g., Bercovici & Karato, 2003; Liu et al., 2016; Schmandt et al., 2014; Tauzin et al., 2010). When melting occurs, a majority of water would strongly partition into the melt. Since the melt is generally mobile, melting near the transition zone regions could lead to large‐ scale transport of water in the Earth's mantle. Therefore, understanding the behavior of hydrogen in mantle minerals is important for our knowledge of the dynamics and evolution of the Earth. A major goal of previous work has been to determine the solubility of water in mantle NAMs at various pres- sures, temperatures, and oxidation states. There has been a reasonable agreement on research results for upper mantle and transition zone minerals (e.g., Karato, 2015; Ohtani, 2015; Peslier et al., 2017). However, water solubility in the lower‐mantle minerals, particularly for bridgmanite, has been poorly con- strained. Previous studies suggested that bridgmanite can contain either low (a few ppm wt, near or less than the detection limit) or high (~2,000 ppm wt) water concentrations (e.g., Bolfan‐Casanova et al., 2003; Inoue et al., 2010; Litasov et al., 2003; Meade et al., 1994; Murakami et al., 2002; Panero et al., 2015). Consequently, the conditions at which melting would occur at the topmost lower mantle by downward flow of transition zone minerals are not well constrained. The cause of large variations in reported water concentrations in bridgmanite is not well known but includes differences in synthesis conditions at high pressure‐temperature (P‐T), compositions and water contents of starting materials, and quenching rates; the use of different analytical techniques and their calibrations; total Fe, Al as well as Fe3+ contents in bridgmanite; and possible contaminations from inclusions of hydrous phases and/or precipitates (e.g., Kaminsky, 2018). In the next two sections, we will present a review to iden- tify possible causes for different results on water solubility in bridgmanite from previous studies. The poten- tial role of inclusions on reported results is emphasized in the discussion below. 1.1. The Use of Analytical Techniques In order to characterize water in mantle minerals, Fourier‐transform infrared spectroscopy (FTIR) and sec- ondary ion mass spectrometry (SIMS) have been commonly used (e.g., Pearson et al., 2014; Sambridge et al., 2008). FTIR can be used to detect characteristic structural OH absorption bands typically in the range of − 3,000–3,800 cm 1. The main advantage of FTIR is that the nature of hydrogen‐related species can be inferred from the frequencies of absorption. Consequently, absorption by inclusions and/or surface contaminants could be distinguished from absorption by hydrogen dissolved in crystallographic sites of the candidate crys- tals. To estimate hydrogen content from IR absorption, one needs reliable calibrations of absorption coeffi- cients in specific crystallographic orientations relative to the polarization direction of the IR beam (Asimow et al., 2006; Aubaud et al., 2007; Balan et al., 2008; Paterson, 1982). However, this calibration standard has not been established yet for bridgmanite. In contrast, SIMS can be used to measure bulk water contents (e.g., Hauri et al., 2011; Kumamoto et al., 2017; Mosenfelder et al., 2011). Nevertheless, in SIMS analyses one cannot distinguish hydrogen in inclusions (e.g., glasses and secondary phases), precipitates, and surface contaminants (e.g., hydroxyls) from hydrogen in crystalline lattices of the sample, if one of these sources is present. 1.2. The Role of Inclusions Experiments on water partitioning between ringwoodite and bridgmanite using multianvil apparatus found that water preferentially partitions into ringwoodite, and ~1–2 ppm wt water was reported to be barely detectable in MgSiO3 or Fe‐bearing bridgmanite using